Prediction of intrinsic two-dimensional ferroelectrics in In2Se3 and other III2-VI3 van der Waals materials

doi:10.1038/ncomms14956

Title: Prediction of intrinsic two-dimensional ferroelectrics in In ₂Se ₃ and other III ₂-VI ₃ van der Waals materials

Interest in two-dimensional (2D) van der Waals materials has grown rapidly across multiple scientific and engineering disciplines in recent years. However, ferroelectricity, the presence of a spontaneous electric polarization, which is important in many practical applications, has rarely been reported in such materials so far. Here we employ first-principles calculations to discover a branch of the 2D materials family, based on In ₂Se ₃ and other III ₂-VI ₃ van der Waals materials, that exhibits room-temperature ferroelectricity with reversible spontaneous electric polarization in both out-of-plane and in-plane orientations. The device potential of these 2D ferroelectric materials is further demonstrated using the examples of van der Waals heterostructures of In ₂Se ₃/graphene, exhibiting a tunable Schottky barrier, and In ₂Se ₃/WSe ₂, showing a significant band gap reduction in the combined system. Lastly, these findings promise to substantially broaden the tunability of van der Waals heterostructures for a wide range of applications.

Authors:

Ding, Wenjun ^[1] ; Zhu, Jianbao ^[2] ; Wang, Zhe ^[1] ; ; Xiao, Di ^[4] ; Gu, Yi ^[5] ; Zhang, Zhenyu ^[6] ; Zhu, Wenguang ^[1]

Univ. of Science and Technology of China, Hefei (China). Dept. of Physics, International Center for Quantum Design of Functional Materials (ICQD), and Key Lab. of Strongly-Coupled Quantum Matter Physics
Univ. of Science and Technology of China, Hefei (China). Dept. of Physics, International Center for Quantum Design of Functional Materials (ICQD), and Key Lab. of Strongly-Coupled Quantum Matter Physics; Beijing Computational Science Research Center, Beijing (China)
Univ. of Tennessee, Knoxville, TN (United States). Dept. of Materials Science and Engineering; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
Carnegie Mellon Univ., Pittsburgh, PA (United States). Dept. of Physics
Washington State Univ., Pullman, WA (United States). Dept. of Physics and Astronomy
Univ. of Science and Technology of China, Hefei (China). International Center for Quantum Design of Functional Materials (ICQD)

Publication Date:: 2017-04-07

Type:: Accepted Manuscript

Journal Name:: Nature Communications

Additional Journal Information:: Journal Volume: 8; Journal ID: ISSN 2041-1723

Publisher:: Nature Publishing Group

Research Org:: Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center

Sponsoring Org:: USDOE

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE

OSTI Identifier:: 1489368


                    Ding, Wenjun, Zhu, Jianbao, Wang, Zhe, Gao, Yanfei, Xiao, Di, Gu, Yi, Zhang, Zhenyu, and Zhu, Wenguang. Prediction of intrinsic two-dimensional ferroelectrics in In2Se3 and other III2-VI3 van der Waals materials.  United States: N. p.,  
        Web.  doi:10.1038/ncomms14956.

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                    Ding, Wenjun, Zhu, Jianbao, Wang, Zhe, Gao, Yanfei, Xiao, Di, Gu, Yi, Zhang, Zhenyu, & Zhu, Wenguang. Prediction of intrinsic two-dimensional ferroelectrics in In2Se3 and other III2-VI3 van der Waals materials.  United States.  doi:10.1038/ncomms14956.

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                    Ding, Wenjun, Zhu, Jianbao, Wang, Zhe, Gao, Yanfei, Xiao, Di, Gu, Yi, Zhang, Zhenyu, and Zhu, Wenguang. 2017.  
        "Prediction of intrinsic two-dimensional ferroelectrics in In2Se3 and other III2-VI3 van der Waals materials".  United States.  
        doi:10.1038/ncomms14956.  https://www.osti.gov/servlets/purl/1489368.

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@article{osti_1489368,

  title        = {Prediction of intrinsic two-dimensional ferroelectrics in In2Se3 and other III2-VI3 van der Waals materials},

  author       = {Ding, Wenjun and Zhu, Jianbao and Wang, Zhe and Gao, Yanfei and Xiao, Di and Gu, Yi and Zhang, Zhenyu and Zhu, Wenguang},

  abstractNote = {Interest in two-dimensional (2D) van der Waals materials has grown rapidly across multiple scientific and engineering disciplines in recent years. However, ferroelectricity, the presence of a spontaneous electric polarization, which is important in many practical applications, has rarely been reported in such materials so far. Here we employ first-principles calculations to discover a branch of the 2D materials family, based on In2Se3 and other III2-VI3 van der Waals materials, that exhibits room-temperature ferroelectricity with reversible spontaneous electric polarization in both out-of-plane and in-plane orientations. The device potential of these 2D ferroelectric materials is further demonstrated using the examples of van der Waals heterostructures of In2Se3/graphene, exhibiting a tunable Schottky barrier, and In2Se3/WSe2, showing a significant band gap reduction in the combined system. Lastly, these findings promise to substantially broaden the tunability of van der Waals heterostructures for a wide range of applications.},

  doi          = {10.1038/ncomms14956},

  journal      = {Nature Communications},

  number       = ,

  volume       = 8,

  place        = {United States},

  year         = {2017},

  month        = {4}

}

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Free Publicly Accessible Full Text
Accepted Manuscript (DOE)
Publisher's Version of Record
10.1038/ncomms14956
https://doi.org/10.1038/ncomms14956

Works referenced in this record:

Ferroelectricity in Ultrathin Perovskite Films
journal, June 2004

Fong, Dillon D.; Stephenson, G. Brian; Streiffer, Stephen K.
Science, Vol. 304, Issue 5677, p. 1650-1653
DOI: 10.1126/science.1098252

Generalized Gradient Approximation Made Simple
journal, October 1996

Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
DOI: 10.1103/PhysRevLett.77.3865

Projector augmented-wave method
journal, December 1994

Bl�chl, P. E.
Physical Review B, Vol. 50, Issue 24, p. 17953-17979
DOI: 10.1103/PhysRevB.50.17953

Van der Waals heterostructures
journal, July 2013

Geim, A. K.; Grigorieva, I. V.
Nature, Vol. 499, Issue 7459, p. 419-425
DOI: 10.1038/nature12385

Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996

Kresse, G.; Furthm�ller, J.
Physical Review B, Vol. 54, Issue 16, p. 11169-11186
DOI: 10.1103/PhysRevB.54.11169

From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999

Kresse, G.; Joubert, D.
Physical Review B, Vol. 59, Issue 3, p. 1758-1775
DOI: 10.1103/PhysRevB.59.1758

Discovery of robust in-plane ferroelectricity in atomic-thick SnTe
journal, July 2016

Chang, Kai; Liu, Junwei; Lin, Haicheng
Science, Vol. 353, Issue 6296, p. 274-278
DOI: 10.1126/science.aad8609

Graphene-Like Two-Dimensional Materials
journal, January 2013

Xu, Mingsheng; Liang, Tao; Shi, Minmin
Chemical Reviews, Vol. 113, Issue 5, p. 3766-3798
DOI: 10.1021/cr300263a

A climbing image nudged elastic band method for finding saddle points and minimum energy paths
journal, December 2000

Henkelman, Graeme; Uberuaga, Blas P.; J�nsson, Hannes
The Journal of Chemical Physics, Vol. 113, Issue 22, p. 9901-9904
DOI: 10.1063/1.1329672

Critical thickness for ferroelectricity in perovskite ultrathin films
journal, April 2003

Junquera, Javier; Ghosez, Philippe
Nature, Vol. 422, Issue 6931, p. 506-509
DOI: 10.1038/nature01501

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Title: Prediction of intrinsic two-dimensional ferroelectrics in In 2Se 3 and other III 2-VI 3 van der Waals materials

Access journal articles and accepted manuscripts
resulting from DOE research funding

Title: Prediction of intrinsic two-dimensional ferroelectrics in In ₂Se ₃ and other III ₂-VI ₃ van der Waals materials